Reaction Dynamics of Excited States of Transition Metal Atoms

过渡金属原子激发态的反应动力学

基本信息

批准号：
14340186
负责人：
HONMA Kenji
金额：
$ 7.74万
依托单位：
Himeji Institute of Technology
依托单位国家：
日本
项目类别：
Grant-in-Aid for Scientific Research (B)
财政年份：
2002
资助国家：
日本
起止时间：
2002 至 2003
项目状态：
已结题

项目摘要

The dynamics of the excited states has been studied experimentally for the reactions involving gas-phase metal atoms. Based on the experimental results, the detail information about potential energy surfaces has been obtained. The crossed-beam technique has been used to achieve the single collision condition, which avoids collisional mixing of electronic states prepared.Metal atoms were generated by the laser vaporization and issued as a metal atomic beam. This beam was crossed with a molecular beam at right angle and reaction products in the crossing region were detected by laser-induced fluorescence (LIF) and/or chemiluminescence techniques. During the term of this project, the following reactions have been studied.Al(^2P_<1/2,3/2>)+O_2(S^3Σ^-_g)→AlO(X^2Σ^+)+O(^3P_J) (1)Y(^2D_<3/2,5/2>)+O_2(X^3Σ^-_g)→YO(X^2Σ^+,A^2Δ_<3/2,5/2>,A^2Π_<1/2,3/2>)+O(^3P_J) (2)Two spin-orbit states were selectively generated and vib-rotational state distributions of AlO were determined for these initial staets. The vacuum ultraviolet LIF technique was employed to determine the populations of three spin-orbit states of the O atom. For both spin-orbit states of Al, the vib-rotational states show almost statistical distribution. This result suggests that the reaction proceeds via a long-lived intermediate. On the other hand, the spin-orbit states of O do not agree with the statistical expectation. This interaction among different spin-orbit states likely to occur at entrance and exit channels of the intermidiate.Chemiluminescence spectra of YO(A^2Π_<1/2,3/2>) were analyzed to determine the energy partition into this product. The vib-rotational state distributions are again almost statistical and a complex mechanism is suggested. The Doppler profiles of the O atom were analyzed to estimate relative branching ratios for YO in the ground state vs. YO in the excited states. The results suggest that more than two pathways take place in reaction (2).

激发态的动力学已通过实验研究了涉及气相金属原子的反应。根据实验结果，已经获得了有关势能表面的详细信息。交叉梁技术已用于实现单个碰撞状态，该条件避免了制备的电子状态的碰撞混合。金属原子是由激光分散剂产生的，并作为金属原子束发行。通过激光诱导的荧光（LIF）和/或化学发光技术检测到交叉区域中的分子束与分子束交叉，并在交叉区域中进行反应产物。在该项目的学期期间，已经进行了以下反应。AL（^2p_ <1/2,3/2>）+O_2（s^3σ^-_ g）→Alo（x^2σ^+）+O（^3p_j） (1)Y(^2D_<3/2,5/2>)+O_2(X^3Σ^-_g)→YO(X^2Σ^+,A^2Δ_<3/2,5/2>,A^2Π_<1/2,3/2>)+O(^3P_J) (2)Two spin-orbit states were selectedly generated and vib-rotational state distributions of AlO were determined for these initial Staets。采用真空紫外线技术来确定O原子的三个自旋轨道状态的种群。对于Al的两个自旋轨道状态，VIB转移状态几乎显示出统计分布。该结果表明该反应通过长期寿命的中间体进行。另一方面，O的自旋轨道状态不同意统计期望。分析了可能发生在中间的入口和出口通道之间的不同自旋轨道状态之间的这种相互作用。分析了YO的化石发光光谱（A^2π_<1/2,3/2>）以确定该产品中的能量分区。旋转状态分布再次几乎是统计的，并提出了复杂的机制。分析了O原子的多普勒轮廓，以估计YO在激发态中基态与YO中的相对分支比率。结果表明反应（2）中发生了两种以上的途径。